Alemayehu Getahun Kumela, Stéphane Lanteri, Francesco Papoff, John Jeffers, Giuseppe Leo, Célestin Lecasble, Jean-Michel Gérard, Mahmoud Elsawy
{"title":"Advanced Multi-Objective Optimization of Nonlinear Metasurface Unlocks Quantum Light Generation","authors":"Alemayehu Getahun Kumela, Stéphane Lanteri, Francesco Papoff, John Jeffers, Giuseppe Leo, Célestin Lecasble, Jean-Michel Gérard, Mahmoud Elsawy","doi":"10.1002/adom.202503793","DOIUrl":"10.1002/adom.202503793","url":null,"abstract":"<div>\u0000 \u0000 <p>The design of nonlinear metasurfaces for quantum applications has traditionally focused on classical figures of merit such as tuning resonances at the pump and target frequencies. While these approaches can enhance nonlinear efficiency, they do not guarantee the precise phase control needed for generating pure quantum state. In this work, we present a hybrid quantum-classical inverse design framework that directly incorporates quantum metrics into the optimization process. By leveraging an advanced multiobjective optimization, we optimized both entanglement fidelity and the spontaneous parametric down conversion (SPDC) rate, ensuring that high brightness and quantum purity are achieved simultaneously. In general, classical methods that rely on bound states in the continuum (BIC) modes or sharp resonances, can improve the SPDC rate but are often sensitive and difficult to control across the polarization channels leading to low quantum purity, uncontrolled correlations, and reduced entanglement fidelity. In contrast, our approach demonstrates that reliable, easy-to-fabricate metasurfaces can achieve superior quantum performance without these constraints. When applied to a [100] AlGaAs nanohole metasurface, our numerical simulations predict a Bell-state fidelity of 0.989 combined with a collected SPDC rate of 55 Hz/mW, integrated over a wide angular emission range. Our optimized design represents a robust architecture for compact, high-purity sources of entangled photon pairs.</p>\u0000 </div>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"14 12","pages":""},"PeriodicalIF":7.2,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147564299","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mengcheng Wang, Hongbing Shi, Di Wu, Li Jiang, Zhijuan Su, Zhuoqing Yang, Guifu Ding, Faheng Zang
{"title":"Enabling Ion Milling Redeposition Nano-Templates for Scalable Nanofabrication of Chemical-Sensing Metamaterials with 10 nm-Feature Size","authors":"Mengcheng Wang, Hongbing Shi, Di Wu, Li Jiang, Zhijuan Su, Zhuoqing Yang, Guifu Ding, Faheng Zang","doi":"10.1002/adom.202600012","DOIUrl":"10.1002/adom.202600012","url":null,"abstract":"<div>\u0000 \u0000 <p>Achieving low-cost patterning of 10 nm-scale nanostructures remains a critical challenge in nanofabrication. Conventional electron beam lithography has a prolonged processing time and limited throughput due to its intrinsic small-area processing nature. Extreme ultraviolet (EUV) lithography faces prohibitive costs in equipment and materials. While industrial nanoimprinting offers a lower-cost, high-throughput alternative, its resolution is fundamentally constrained by the template's minimum feature size. Herein, we present a new nanofabrication process that exploits the redeposition effect in ion milling to fabricate controllable 10 nm-scale nanogaps. This approach enabled the preparation of gratings and nanorings array integrated with noble metal nanogaps for applications in surface-enhanced Raman spectroscopy (SERS). Furthermore, gratings and nanopillar arrays with sidewalls coated by a metal mask were dry-etched to form a self-aligned stacked nanomorphology on a silicon substrate without optical alignment, inheriting the metal mask's minimum feature size. The resulting high-quality templates subsequently facilitated high-fidelity replication of diminutive structures via nanoimprint lithography (NIL). This scalable strategy holds significant potential as a feasible route for manufacturing applications in nanophononics, biosensing, quantum devices, integrated circuits (ICs), and beyond.</p>\u0000 </div>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"14 12","pages":""},"PeriodicalIF":7.2,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147564815","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Po-Hsien Lai, Chien-Cheng Li, Tien-Lin Wu, Chih-Shan Tan
{"title":"ZnCl2 Post-Treatment Enables High-Efficiency Violet CsPbCl3 Quantum Dot LEDs","authors":"Po-Hsien Lai, Chien-Cheng Li, Tien-Lin Wu, Chih-Shan Tan","doi":"10.1002/adom.202503635","DOIUrl":"10.1002/adom.202503635","url":null,"abstract":"<p>Perovskite light-emitting diodes (LEDs) have achieved external quantum efficiencies (EQEs) above 20% in the red, green, and blue spectral regions, yet their efficiency rapidly declines as the bandgap widens for shorter-wavelength emission. This limitation hampers the development of high-bandgap perovskite LEDs, including ultraviolet (UV) devices. Here, we report efficiency enhancement in violet-emitting perovskite quantum dot LEDs through ZnCl<sub>2</sub> post-treatment doping as a step toward future UV LED technologies. ZnCl<sub>2</sub> doping significantly improves optoelectronic performance, increasing the EQE from 0.38% to 0.90%, raising the maximum luminance from 95.29 to 156.39 cd/m<sup>2</sup>, and reducing the turn-on voltage from 3.88 to 3.65 V. These results indicate that ZnCl<sub>2</sub> post-treatment effectively enhances carrier transport and overall device performance, offering a promising strategy to enable efficient high-bandgap perovskite LEDs.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"14 12","pages":""},"PeriodicalIF":7.2,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/adom.202503635","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147565360","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Exploration of Pyridyl Porphyrin as Ultrafast Hot Hole Extractor From Colloidal CsPbI3 Quantum Dots","authors":"Sadashiv Wadepalli, Shekhar Mondal, Souvik Das, Naga Pranava Sree Kothoori, Pralok K. Samanta, Prakriti Ranjan Bangal, Abhijit Hazarika","doi":"10.1002/adom.202503615","DOIUrl":"10.1002/adom.202503615","url":null,"abstract":"<div>\u0000 \u0000 <p>Metal halide perovskites (MHPs) have intrinsically slow hot carrier (HC) cooling, and by tethering suitable extractors, photoexcited HCs can effectively be harvested. This enables the utilization of excess carrier energy before thermalization which is crucial to surpass the thermodynamic limit of energy conversion efficiency in photovoltaic devices. The HC cooling process can further be slowed down in MHP quantum dots (QDs) due to energy discretization. Here, we demonstrate efficient room-temperature hot-hole extraction from CsPbI<sub>3</sub> (CPI) QDs, a narrow bandgap MHP composition, to energetically favourable 5,10,15,20-tetra(4-pyridyl) porphyrin (TPyP). Steady-state and time-resolved photoluminescence studies reveal dynamic photoluminescence quenching which is attributed to the strong binding affinity of the TPyP molecules to the CPI QD surface. Employing transient absorption spectroscopy (<i>fs</i>-TAS), we show that there is a significant lowering of the hot-hole cooling time of these QDs from ∼900 to ∼700 fs in the presence of TPyP, and the average hot-hole extraction efficiency was estimated to be ∼22%. Further, we demonstrate hot hole extraction in electronically coupled CPI QD solid films to a TPyP layer with an efficiency of ∼29%. These results emphasize the need to explore the coupling of PQDs and macrocyclic molecules to harness photoexcited HCs, which can potentially help in designing next-generation photovoltaic devices.</p>\u0000 </div>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"14 12","pages":""},"PeriodicalIF":7.2,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147566144","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Bangqi Jiang, Wen Yang, Yao Xiao, Ziyue Rao, Yugeng Hao, Ruijiang Hong
{"title":"A Multi-Additive System With Superimposed Optimization Effects by Incorporating Additives With Tailored Mechanisms for Perovskite Solar Cells","authors":"Bangqi Jiang, Wen Yang, Yao Xiao, Ziyue Rao, Yugeng Hao, Ruijiang Hong","doi":"10.1002/adom.202503859","DOIUrl":"10.1002/adom.202503859","url":null,"abstract":"<div>\u0000 \u0000 <p>Perovskite/c-Si tandem solar cells have emerged as one of the most promising candidates for next-generation solar cells in recent years. However, the wide-bandgap (1.65–1.70 eV) perovskite top cells still encounter numerous challenges, such as suboptimal crystallization quality, poor stability, and interface recombination losses. In this study, the effects of four types of additives (i.e., MACl & Pb-excess, ODADI, PMMA, and Me-4PACz) co-added to perovskite were investigated. Multiple mechanisms including intermediate phase-assisted α-phase formation, Pb anchoring, grain boundary passivation and interface modification have been discovered. Due to different interaction mechanisms and distribution areas, the optimized effects of these additives can be superimposed without interference with each other. Consequently, the crystallinity of perovskite film was optimized, the precipitation of Pb was suppressed, and the deep defect density was reduced, thus shifting the dominant recombination defect type from deep defects to shallow defects, significantly reducing non-radiative recombination. The best PSCs (E<sub>g</sub> = 1.694 eV) fabricated through the co-addition strategy with PCE = 21.50%, SPO = 20.73%, and stability T<sub>90</sub> ≈ 480 h (storage conditions: 30% humidity, 25°C) were obtained. Our research demonstrated the application potential of the multi-additive system for the additive engineering of perovskites.</p>\u0000 </div>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"14 12","pages":""},"PeriodicalIF":7.2,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147563521","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Adam Bickerdike, Mahdiyar Nouri-Rezaie, Takuji Hatakeyama, Chris Groves, Chihaya Adachi, Mujeeb U. Chaudhry, Roderick C. I. MacKenzie
{"title":"Reverse Intersystem Crossing and Exciton Harvesting: A Pathway to Low Threshold in Multi-Resonant TADF Electrically Pumped Organic Semiconductor Lasers","authors":"Adam Bickerdike, Mahdiyar Nouri-Rezaie, Takuji Hatakeyama, Chris Groves, Chihaya Adachi, Mujeeb U. Chaudhry, Roderick C. I. MacKenzie","doi":"10.1002/adom.202501796","DOIUrl":"10.1002/adom.202501796","url":null,"abstract":"<p>If electrically pumped lasing in organic semiconductors could be achieved, it would have a wide-ranging impact on many fields, including healthcare, information transmission, and sensing to name a few. However, a major challenge in the development of these devices is overcoming triplet accumulation that leads to the annihilation of the lasing singlet species. The utilization of triplet recycling, whereby triplets are back converted into lasing singlets has emerged as a promising strategy to address this. Herein, high-speed micro-OLEDs incorporating the multi-resonant TADF emitter DABNA-2 are found to exhibit marked performance enhancements upon introduction into a BSBCz host, which serves as an efficient triplet scavenger. This tailored host environment demonstrates a path to low-threshold lasing devices. Using a combination of experiment and numerical modelling, we visualize the build up of the singlets/triplets/polarons within the device identifying key mechanisms that can be used to reduce the lasing threshold. Using this framework, we are able to calculate lasing thresholds for these materials and estimate how far the community is from a lasing device.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"14 12","pages":""},"PeriodicalIF":7.2,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/adom.202501796","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147566143","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Ratiometric Temperature Sensing through Alternating Current Electroluminescence","authors":"Zhifeng Xing, Shuohan Li, Xin Zhang, Fengjun Chun, Yaxin Cao, Shengqiang Liu, Xiaohe Wei, Feng Wang","doi":"10.1002/adom.202503425","DOIUrl":"10.1002/adom.202503425","url":null,"abstract":"<p>Thermoresponsive luminescent materials have been developed over the past decades for temperature monitoring in diverse scenarios. However, traditional luminescence thermometers typically require excitation by light sources such as lasers and light-emitting diodes, which may suffer from errors caused by uneven distribution of the excitation light and environmental interference. In this report, ZnS doped with Cu<sup>+</sup> and Cl<sup>−</sup> is investigated for electroluminescence thermometry driven by alternating current. The ZnS:Cu/Cl generates blue-green dual emissions, which exhibit dissimilar responses to temperature changes, giving rise to the thermometric property. The thermometric performance is further improved by refining the thermal response of the green emission through Co<sup>2+</sup> tri-doping, registering a relative sensitivity of 1.19% K<sup>−1</sup> at around 50°C. The advances in these alternating-current-driven thermoresponsive optical materials offer exciting opportunities for quantitative temperature detection and visualized surface temperature mapping.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"14 12","pages":""},"PeriodicalIF":7.2,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/adom.202503425","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147563302","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Viola Bauernfeind, Viola V. Vogler-Neuling, Ilja Gunkel, Primož Pirih, Ullrich Steiner, Bodo D. Wilts
{"title":"Optical Diversity and Nanostructural Organization in the Colored Scales of Sternotomis","authors":"Viola Bauernfeind, Viola V. Vogler-Neuling, Ilja Gunkel, Primož Pirih, Ullrich Steiner, Bodo D. Wilts","doi":"10.1002/adom.202503324","DOIUrl":"10.1002/adom.202503324","url":null,"abstract":"<p>Many longhorn beetles display vibrant color patterns that arise from a combination of pigmentary absorption and light interference with photonic structures within nanostructured scales. This study provides a comprehensive overview of the optical properties of the colored scales in 22 species of the genus <i>Sternotomis</i> (Cerambycidae: Lamiinae: Sternotomini; Percheron, 1836) using reflectance spectroscopy, scanning electron microscopy, and small-angle X-ray scattering (SAXS). While individual species of this genus have been studied in detail, a systematic comparison of optical signatures and underlying photonic architectures across the entire genus has been lacking. The diversity of color-producing mechanisms within the genus reveals significant variations in scale structuring and pigment colors, accompanied by noticeable changes in local nanostructural motifs. This study establishes a spectral–structural framework for understanding controlled disorder in biological photonic materials and lays the groundwork for research on the development of biological photonic systems with controlled disorder and diverse optical properties.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"14 12","pages":""},"PeriodicalIF":7.2,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/adom.202503324","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147566148","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Achieving High Photoluminescence Quantum Yield in Sb-Doped Indium-Based Hybrid Halides for Single-Component Warm White LEDs","authors":"Yuyang He, Yuting Xu, Yuzhen Wang, Shuai Zhang, Zhiguo Xia","doi":"10.1002/adom.202600001","DOIUrl":"10.1002/adom.202600001","url":null,"abstract":"<div>\u0000 \u0000 <p>Indium(III)-based hybrid halides are emerging low-dimensional luminescent materials; however, their rigid lattices and <i>d</i><sup>10</sup> electronic configuration of In<sup>3+</sup> suppress intrinsic self-trapped-exciton (STE) emission, leading to limited photoluminescence quantum yield (PLQY). To address this issue, Sb<sup>3+</sup> is doped into the 0D (Me<sub>2</sub>NH<sub>2</sub>)<sub>4</sub>InCl<sub>7</sub> host, transforming it from a nearly non-emissive material into a highly efficient warm-white STE emitter. The optimized (Me<sub>2</sub>NH<sub>2</sub>)<sub>4</sub>InCl<sub>7</sub>:0.2Sb<sup>3+</sup> delivers a near-unity PLQY (∼100%) under 350 nm excitation. Single-crystal structural analysis and theoretical calculations reveal substitutional Sb<sup>3+</sup> at In<sup>3+</sup> sites, inducing locally distorted [SbCl<sub>6</sub>] octahedra. This Sb<sup>3+</sup>-triggered local lattice distortion strengthens electron–phonon coupling, and it deepens the STE potential well and suppresses non-radiative relaxation pathways, thereby enabling robust broadband STE emission with a microsecond-scale lifetime (4.28 µs), a large Stokes shift (280 nm), and a wide bandwidth (177 nm). This work provides a facile route to realize warm-white emission from a single host lattice based on stable, low-toxicity indium-based hybrid halides.</p>\u0000 </div>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"14 12","pages":""},"PeriodicalIF":7.2,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147563306","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Aleksandra D. Valueva, Emily M. Chopra, Vladislav V. Klepov
{"title":"Unraveling Mechanism of Photoluminescence in Hybrid Indium Halide Materials","authors":"Aleksandra D. Valueva, Emily M. Chopra, Vladislav V. Klepov","doi":"10.1002/adom.202600007","DOIUrl":"10.1002/adom.202600007","url":null,"abstract":"<p>Indium-based hybrid halides are promising lead-free luminescent materials, yet the design principles for these closed-shell ns<sup>0</sup> systems remain underdeveloped compared to traditional ns<sup>2</sup> analogues. Here, we synthesized and characterized the (Pr<sub>2</sub>NH<sub>2</sub>)<sub>3</sub>In(Cl<sub>1-x</sub>Br<sub>x</sub>)<sub>6</sub> (0 ≤ x ≤ 1) solid-solution series to unravel their halide-dependent effects. Combined spectroscopic and DFT analyses confirm that photoluminescence originates from ligand-to-metal charge transfer (LMCT) excitation followed by radiative recombination from self-trapped excitons (STEs). The systematic substitution of halides induces a non-monotonic red shift in emission energy that plateaus beyond x ≥ 0.3, while the photoluminescence quantum yield (PLQY) increases monotonically with bromide content, reaching up to 70% for (Pr<sub>2</sub>NH<sub>2</sub>)<sub>3</sub>In(Cl<sub>0.2</sub>Br<sub>0.8</sub>)<sub>6</sub>. These trends are rationalized by the electronic isolation of [InHal<sub>6</sub>]<sup>3−</sup> units and increased lattice softness in bromide-rich compositions, which facilitates radiative STE formation. Our work establishes a coherent mechanistic foundation for indium halide hybrids, demonstrating how halide identity and electronic isolation dictate radiative processes in efficient lead-free emitters.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":"14 12","pages":""},"PeriodicalIF":7.2,"publicationDate":"2026-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/adom.202600007","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147563307","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}